US5235804A - Method and system for combusting hydrocarbon fuels with low pollutant emissions by controllably extracting heat from the catalytic oxidation stage - Google Patents
Method and system for combusting hydrocarbon fuels with low pollutant emissions by controllably extracting heat from the catalytic oxidation stage Download PDFInfo
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- US5235804A US5235804A US07/701,426 US70142691A US5235804A US 5235804 A US5235804 A US 5235804A US 70142691 A US70142691 A US 70142691A US 5235804 A US5235804 A US 5235804A
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Classifications
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F23—COMBUSTION APPARATUS; COMBUSTION PROCESSES
- F23C—METHODS OR APPARATUS FOR COMBUSTION USING FLUID FUEL OR SOLID FUEL SUSPENDED IN A CARRIER GAS OR AIR
- F23C13/00—Apparatus in which combustion takes place in the presence of catalytic material
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F02—COMBUSTION ENGINES; HOT-GAS OR COMBUSTION-PRODUCT ENGINE PLANTS
- F02B—INTERNAL-COMBUSTION PISTON ENGINES; COMBUSTION ENGINES IN GENERAL
- F02B51/00—Other methods of operating engines involving pretreating of, or adding substances to, combustion air, fuel, or fuel-air mixture of the engines
- F02B51/02—Other methods of operating engines involving pretreating of, or adding substances to, combustion air, fuel, or fuel-air mixture of the engines involving catalysts
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F02—COMBUSTION ENGINES; HOT-GAS OR COMBUSTION-PRODUCT ENGINE PLANTS
- F02M—SUPPLYING COMBUSTION ENGINES IN GENERAL WITH COMBUSTIBLE MIXTURES OR CONSTITUENTS THEREOF
- F02M27/00—Apparatus for treating combustion-air, fuel, or fuel-air mixture, by catalysts, electric means, magnetism, rays, sound waves, or the like
- F02M27/02—Apparatus for treating combustion-air, fuel, or fuel-air mixture, by catalysts, electric means, magnetism, rays, sound waves, or the like by catalysts
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F23—COMBUSTION APPARATUS; COMBUSTION PROCESSES
- F23C—METHODS OR APPARATUS FOR COMBUSTION USING FLUID FUEL OR SOLID FUEL SUSPENDED IN A CARRIER GAS OR AIR
- F23C6/00—Combustion apparatus characterised by the combination of two or more combustion chambers or combustion zones, e.g. for staged combustion
- F23C6/04—Combustion apparatus characterised by the combination of two or more combustion chambers or combustion zones, e.g. for staged combustion in series connection
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F23—COMBUSTION APPARATUS; COMBUSTION PROCESSES
- F23R—GENERATING COMBUSTION PRODUCTS OF HIGH PRESSURE OR HIGH VELOCITY, e.g. GAS-TURBINE COMBUSTION CHAMBERS
- F23R3/00—Continuous combustion chambers using liquid or gaseous fuel
- F23R3/40—Continuous combustion chambers using liquid or gaseous fuel characterised by the use of catalytic means
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
- Y02T10/00—Road transport of goods or passengers
- Y02T10/10—Internal combustion engine [ICE] based vehicles
- Y02T10/12—Improving ICE efficiencies
Definitions
- the present invention relates to a method and system for combusting hydrocarbon fuels with low pollutant emissions, particularly low NO x emissions.
- exhaust gases produced by combusting hydrocarbon fuels can contribute to atmospheric pollution.
- Exhaust gases typically contain pollutants such as nitric oxide (NO) and nitrogen dioxide (NO 2 ), which are frequently grouped together as NO x , unburned hydrocarbons (UHC), carbon monoxide (CO), and particulates, primarily carbon soot.
- NO x may be formed by several mechanisms. The high temperature reaction of atmospheric oxygen with atmospheric nitrogen, particularly at adiabatic flame temperatures above about 2800° F., forms NO x through the thermal or the Zeldovich mechanism ("thermal NO x ").
- An equivalence ratio of greater than 1.0 indicates fuel-rich conditions, while an equivalence ratio of less than 1.0 indicates fuel-lean conditions.
- Burning a fuel at an equivalence ratio slightly less than 1.0 produces nearly complete combustion, minimizing CO and UHC production, and a hot flame, maximizing useable energy.
- the temperatures produced during such an operation are high enough to produce appreciable quantities of thermal NO x . Therefore, the goal of achieving good thermal efficiency, which arises from economic concerns, is seemingly at odds with the goal of minimizing NO x emissions, which arises from environmental concerns and is required by increasingly stringent environmental regulations.
- thermal NO x can be reduced by operating under uniformly fuel-lean conditions, such as by using a lean diffusion flame or a lean premixed/prevaporized (LPP) system.
- LPP lean premixed/prevaporized
- the formation of prompt NO x can also be reduced by operating under fuel-lean conditions because the excess air decreases the concentration of CH i available to react with atmospheric nitrogen.
- the extent to which thermal and prompt NO x formation can be reduced by fuel-lean combustion may be limited by flame instability which occurs at very lean conditions.
- One aspect of the invention includes a method of combusting a hydrocarbon fuel.
- the fuel is mixed with a first air stream to form a fuel/air mixture having an equivalence ratio greater than 1 and partially oxidized by contacting the fuel/air mixture with an oxidation catalyst in a catalytic oxidation stage, thereby generating a heat of reaction and a partial oxidation product stream comprising hydrogen and carbon oxides.
- the partial oxidation product stream is mixed with a second air stream and completely combusted in a main combustor at a condition at which appreciable quantities of thermal NO x are not formed, thereby generating an effluent gas stream containing decreased amounts of thermal and prompt NO x .
- FIG. 1 is a schematic representation of a basic combustion system of the present invention.
- FIG. 2 is a schematic representation of a combustion system of the present invention used in conjunction with a gas turbine engine.
- the present invention uses a combination of three approaches, partial oxidation by catalytic means, thermal management, and flame stability enhancement to control NO x and other pollutant emissions while permitting thermally efficient combustion of hydrocarbon fuels in a wide variety of combustion devices including residential heating units, industrial process heaters, industrial gas turbines, aircraft gas turbines, and advanced aircraft engines such as those contemplated for the high speed civil transport and national aerospace plane projects.
- FIG. 1 is a schematic of a basic embodiment of the present invention.
- Suitable liquid fuels include kerosine, No. 1 heating oil, No. 2 heating oil, and conventional aviation turbine fuels such as Jet A, Jet B, JP-4, JP-5, JP-7, and JP-8. If the fuel is a liquid, it should be vaporized or atomized before mixing with the air or while being mixed with the air. Any conventional means known in the art may be used to vaporize or atomize the fuel.
- Partially oxidizing the fuel to H 2 , CO, and other carbon oxides by catalytic means reduces the amount of hydrocarbon fuel available to form CH i fragments in a downstream thermal combustor flame front and therefore, reduces the amount of prompt NO x formed in downstream combustion.
- the amount of H 2 , CO, and unreacted hydrocarbon fuel actually formed depends on the temperature in the catalytic oxidation stage, which may range from about 300° F. to about 1800° F. At higher temperatures, relatively more fuel is converted to H 2 and CO than at lower temperatures due to changes in the equilibrium product composition.
- the oxidation catalyst may be any catalyst capable of partially oxidizing the fuel.
- Suitable catalysts include platinum family metals such as platinum, rhodium, iridium, ruthenium, palladium, and mixtures thereof; chromium oxides; cobalt oxides; and alumina.
- the catalyst will be capable of initiating the partial oxidation reaction at the conditions prevailing in the catalytic oxidation stage, that is, without the addition of heat from an external source.
- the catalyst may be preheated using a secondary working fluid, resistive heating, or temporary thermal combustion upstream of the catalyst.
- the catalyst may be supported on alumina or a similar substrate and may be in any conventional form, including granules, extrudates, or a coating on a metal heat exchanger surface, metal foil, metal honeycomb, or ceramic honeycomb.
- the preferred catalysts include platinum family metals, especially platinum-rhodium deposited on an alumina support. If desired, more than one catalyst may be incorporated into a graded catalyst bed.
- the catalytic oxidation stage may be designed according to conventional catalytic reactor design techniques.
- any increase in prompt NO x resulting from the larger amount of unreacted hydrocarbon fuel will be at least partially offset by a reduction in thermal NO x formed in a downstream thermal combustor where the cooler partial oxidation product stream produces a lower adiabatic flame temperature.
- thermal management may be used to extract up to about 50% of the heat of reaction generated in the catalytic oxidation stage. Preferably, up to about 20% of the heat of reaction will be extracted and, most preferably, about 3% to about 20% of the heat of reaction will be extracted.
- the heat extraction may take place downstream of the catalytic oxidation stage, in which case only the temperature of the partial oxidation product stream 12 may be controlled.
- a heat exchanger may be used to extract a portion of the heat of reaction.
- the heat exchanger may be designed according to conventional heat exchanger design techniques and may be an integral part of the catalytic oxidation stage or may be a separate unit.
- the heat transfer stream 14 may initially be at any temperature which permits heat to be extracted from the catalytic oxidation stage or partial oxidation product stream, while its temperature after thermal management will depend on the amount of heat extracted.
- the heat transfer stream 14 may be air, water, or another medium and, after thermal management, can be used in any capacity for which a person skilled in the art would consider such a heated stream to be useful. Effective use of the heat transfer stream 14 permits the thermal efficiency of the present invention to be at least as good as a conventional combustion system.
- the cooled partial oxidation product stream 12 is mixed with the second air stream 6 in a main combustor and is completely combusted by a thermal combustion reaction, generating an exhaust gas stream 16.
- the cooled partial oxidation product stream may be mixed with the second air stream prior to combustion or in a diffusion flame.
- the adiabatic flame temperature in the main combustor will be less than about 2800° F. to minimize the formation of thermal NO x .
- the adiabatic flame temperature and flame stability characteristics in the main combustor depend on the temperature and composition of the partial oxidation product stream and the equivalence ratio in the combustor.
- the H 2 in the partial oxidation product stream enhances flame stability because H 2 is lighter and more reactive than the original fuel and mixes better with the second air stream. Flame stability is especially enhanced when little or no heat is extracted from the catalytic oxidation stage because the partial oxidation product stream will contain more H 2 and will be hotter, leading to better mixing.
- a more stable flame permits the main combustor to be operated at a lower equivalence ratio, which produces a lower adiabatic flame temperature and less thermal NO x . In any case, the main combustor should be operated at an overall equivalence ratio of less than 1.0 to ensure complete combustion.
- the main combustor may be any combustor suitable for combusting the partial oxidation product stream, including a conventional or advanced combustor, and may have either a single combustion zone or a plurality of combustion zones.
- the main combustor will be a lean premixed prevaporized combustor.
- the main combustor may be designed according to conventional techniques.
- Air stream 22 enters a compressor and is compressed to a suitable temperature and pressure.
- the air exiting the compressor is controllably divided into three streams, a first air stream 24, a primary air stream 26, and a secondary air stream 28.
- the first air stream 24 mixes with a fuel stream 30 to form a fuel/air mixture 32 having an equivalence ratio greater than 1.0.
- the fuel/air mixture 32 enters a catalytic oxidation stage where it is contacted with an oxidation catalyst 33 and partially oxidized to produce a heat of reaction and a partial oxidation product stream 34 comprising H 2 and carbon oxides.
- a portion of the heat of reaction is removed in a heat exchanger by the secondary air stream 28, heating the secondary air stream 28 and cooling the partial oxidation product stream 34.
- the cooled partial oxidation product stream 34 mixes with the primary air stream 26 and is thermally combusted in a primary zone of a main combustor at a temperature at which appreciable quantities of thermal NO x are not formed to generate a combustion product stream 36.
- the fuel/air equivalence ratio in the primary zone may be greater than 1.0, or less than 1.0, but preferably, will be less than 1.0 to minimize both thermal and prompt NO x formation.
- a system such as that depicted in FIG. 2 can provide gas turbines with significant additional operating flexibility, particularly when the turbines are operated off peak power.
- the improved flame stability provided by burning a lighter, more reactive fuel in the main combustor provides wider flammability limits than are available from other fuels, permitting combustion to be maintained at lower equivalence ratios.
- the ability to control the division of the air stream into a primary stream and a secondary stream can be used to provide dynamic control of the equivalence ratio in the primary zone so that it is kept constant as power levels are changed.
- a gas turbine engine incorporating a catalytic oxidation stage and a two zone main combustor as shown in FIG. 2 was modelled on a computer using conventional techniques which are well known in the art.
- the catalytic oxidation stage was represented by a detailed chemical kinetic model
- the main combustor primary zone was represented by a perfectly stirred reactor
- the main combustor secondary zone was represented by a plug flow reactor.
- Compressed air at 18.9 atmospheres and 847° F. was split into three streams: 7.5% of the air to the first air stream, 42.5% of the air to the primary air stream, and 50% of the air to the secondary air stream.
- the first air stream was mixed with methane, which was at 80° F., to form a fuel/air mixture which had an equivalence ratio of 4.0 and a temperature of 564° F.
- the fuel/air mixture was partially oxidized in the catalytic oxidation stage to produce a partial oxidation product stream comprising 12 volume percent (vol %) CH 4 , 8 vol % CO, and 19 vol % H 2 .
- the residence time in the catalytic oxidation stage was 20 milliseconds (msec) and the temperature was maintained at 1340° F. by using thermal management to heat the secondary air stream to 1192° F.
- the partial oxidation product stream which exited the catalytic stage at 1340° F., was mixed with the primary air stream in the main combustor primary zone and thermally combusted with a residence time of 0.1 msec and an equivalence ratio of 0.6.
- the combustion product stream which was at 2750° F. and contained 6 parts per million (ppm) NO and 6,000 ppm CO, was mixed with the secondary air stream in the main combustor secondary zone with a residence time of 6.0 msec and an equivalence ratio of 0.3 to produce an exhaust gas stream.
- the exhaust gas stream exited the secondary zone at 2049° F. and contained 3 ppm NO and 6 ppm CO.
- Example 1 The model from Example 1 was used to model a range of operations in the main combustor. Conditions in the catalytic oxidation stage were maintained at 1250° F. and an equivalence ratio of 4 for all cases. Methane and natural gas were used as the fuels for this example. The equivalence ratio in the primary zone was varied from 0.6 to 1.5 and the adiabatic flame temperature was permitted to vary accordingly. The equivalence ratio in the secondary zone was fixed at 0.3. A model of a prior art combustion system with an identical main combustor but lacking a catalytic oxidation stage was also prepared.
- FIG. 3 demonstrates that the present invention can reduce NO x emission levels by a factor of three to five at a given equivalence ratio and can reduce adiabatic flame temperatures by several hundred degrees at a given equivalence ratio.
- the present invention is capable of providing several benefits over the prior art.
- First, it provides three techniques, partial oxidation by catalytic means, thermal management, and flame stabilization, by which NO x and other pollutant emissions can be reduced while maintaining good thermal efficiency.
- the extent to which any of the three techniques is used can be varied to optimize the combustion system operation and design.
- the ability to control the amount of air directed to the primary and secondary zones of the main combustor permits dynamic control of the equivalence ratio in the primary zone for off peak operations. Such a control scheme would be particularly beneficial in gas turbines.
- the present invention has the flexibility to be used with rich-burn-quench-lean-burn, or other advanced combustion techniques to further reduce NO x emissions.
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Abstract
Description
Claims (18)
Priority Applications (6)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
US07/701,426 US5235804A (en) | 1991-05-15 | 1991-05-15 | Method and system for combusting hydrocarbon fuels with low pollutant emissions by controllably extracting heat from the catalytic oxidation stage |
PCT/US1992/003771 WO1992020963A1 (en) | 1991-05-15 | 1992-05-05 | Method and system for combusting hydrocarbon fuels with low pollutant emissions |
AU21540/92A AU654377B2 (en) | 1991-05-15 | 1992-05-05 | Method and system for combusting hydrocarbon fuels with low pollutant emissions |
JP50007493A JP3401246B2 (en) | 1991-05-15 | 1992-05-05 | Method and system for burning hydrocarbon fuel |
DE69201563T DE69201563T2 (en) | 1991-05-15 | 1992-05-05 | METHOD AND SYSTEM FOR HYDROCARBON COMBUSTION WITH LOW POLLUTANT EMISSIONS. |
EP92913087A EP0584263B1 (en) | 1991-05-15 | 1992-05-05 | Method and system for combusting hydrocarbon fuels with low pollutant emissions |
Applications Claiming Priority (1)
Application Number | Priority Date | Filing Date | Title |
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US07/701,426 US5235804A (en) | 1991-05-15 | 1991-05-15 | Method and system for combusting hydrocarbon fuels with low pollutant emissions by controllably extracting heat from the catalytic oxidation stage |
Publications (1)
Publication Number | Publication Date |
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US5235804A true US5235804A (en) | 1993-08-17 |
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Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
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US07/701,426 Expired - Lifetime US5235804A (en) | 1991-05-15 | 1991-05-15 | Method and system for combusting hydrocarbon fuels with low pollutant emissions by controllably extracting heat from the catalytic oxidation stage |
Country Status (6)
Country | Link |
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US (1) | US5235804A (en) |
EP (1) | EP0584263B1 (en) |
JP (1) | JP3401246B2 (en) |
AU (1) | AU654377B2 (en) |
DE (1) | DE69201563T2 (en) |
WO (1) | WO1992020963A1 (en) |
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Also Published As
Publication number | Publication date |
---|---|
WO1992020963A1 (en) | 1992-11-26 |
AU2154092A (en) | 1992-12-30 |
AU654377B2 (en) | 1994-11-03 |
JPH06507957A (en) | 1994-09-08 |
JP3401246B2 (en) | 2003-04-28 |
EP0584263A1 (en) | 1994-03-02 |
DE69201563D1 (en) | 1995-04-06 |
DE69201563T2 (en) | 1995-11-09 |
EP0584263B1 (en) | 1995-03-01 |
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